Hybrid Hydrogels with Orthogonal Transient Cross-linking Exhibiting Highly Tunable Mechanical Properties

Houben, Sofie; Aldana, Ana Agustina; Huysecom, An-Sofie; Mpinganzima, Winy; Cardinaels, Ruth; Baker, Matthew B.; Pitet, Louis M.

doi:10.1021/acsapm.2c01906

Cited by 6 publications

(1 citation statement)

References 48 publications

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“…[24,25] To overcome the low viscosity and the lack of print fidelity, post-printing modifications are engineered into the hydrogel systems to stabilize the 3D structures and prevent the dissolution of the gel under wet conditions as in most biomedical applications. To address these issues, interpenetrating network (IPN) formation [25][26][27][28] became a popular and promising approach. In a typical procedure, the IPN is formed using different crosslinking reactions to create one flexible primary network and one stiff secondary network that have limited interactions with each other.…”

Section: Introductionmentioning

confidence: 99%

Cucurbit[8]uril Mediated Supramolecular and Photocrosslinked Interpenetrating Network Hydrogel Matrices for 3D‐Bioprinting

Wang,

Bimmermann,

Neufurth

et al. 2024

Advanced Materials

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Printing of biologically functional constructs is significant for applications in tissue engineering and regenerative medicine. Designing bio‐inks remains remarkably challenging due to the multifaceted requirements in terms of the physical, chemical and biochemical properties of the three‐dimensional matrix, such as cytocompatibility, printability and shape fidelity. In order to promote matrix and materials stiffness, while not sacrificing stress relaxation mechanisms which support cell spreading, migration and differentiation, we report an interpenetrating network bio‐ink design. Our approach makes use of a chemically defined network, combining physical and chemical crosslinking unites with a tunable composition and network density, as well as spatiotemporal control over post‐assembly material stiffening. To this end, star‐shaped polyethylene glycols functionalized with Phe‐Gly‐Gly tripeptide or photoactive stilbazolium are synthesized, and used to prepare three‐dimensional networks with cucurbit[8]uril (CB[8]) through supramolecular host‐guest‐complexation. The hydrogel obtained shows fast relaxation and thus supports the proliferation and differentiation of cells. Upon irradiation, the mechanical properties of the hydrogel can be rapidly adapted via selective photochemical dimerization of stilbazolium within CB[8], leading to interpenetrating networks with increased form stability while retaining the dynamic nature of the hydrogels. This modular approach opens new design opportunities for extrudable and cell‐friendly dynamic biomaterials for applications in 3D‐bioprinting.This article is protected by copyright. All rights reserved

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Section: Introductionmentioning

confidence: 99%

Cucurbit[8]uril Mediated Supramolecular and Photocrosslinked Interpenetrating Network Hydrogel Matrices for 3D‐Bioprinting

Wang,

Bimmermann,

Neufurth

et al. 2024

Advanced Materials

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Supramolecular hydrogels based on hydrogen bonding: Impact of ionic comonomers

Jangizehi,

Sprenger,

Seiffert

2024

Journal of Polymer Science

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The polymerization of N‐acryloyl glycineamide (NAGA) in water results in the creation of robust supramolecular hydrogels, exhibiting a network structure through inter‐chain crosslinking formed by hydrogen bonds between NAGA units. The stability of these hydrogen bonds in water is based on the aggregation of NAGA units into microdomains or clusters, thereby effectively shielding the hydrogen bonds from the surrounding aqueous medium. Beyond the inherent water absorption characteristics of these hydrogels, the unique ability for the dissociation and re‐association of their physical crosslinks imparts features such as reversible swelling and shrinking as well as self‐healing and remolding capabilities. In this study, we synthesize a series of supramolecular hydrogels through copolymerization of NAGA and ionic sodium acrylate comonomers for a dual purpose: first, to regulate water absorption levels, and second, to introduce a salt partitioning effect into the hydrogels during their swelling in salt solution. Our findings indicate that the properties of these hydrogels are intricately influenced by the volume fraction of the solid network, the concentration of ionic units, and temperature. Notably, supramolecular samples with ionic units exhibit a 16% salt rejection in a single cycle of salt partitioning during their swelling in a 1 g·L−1 sodium chloride solution.

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A new PVA-κCA double-network hydrogel comprising conductive polyaniline nanofibers for strain sensing applications

Al-Goraee,

Alshorman,

Bozeya

et al. 2024

emergent mater.

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Wearable and flexible materials are replacing the conventional solid-state sensors in diffident biomedical applications. Hydrogel-based sensing elements offer several appealing inherent properties such as tissue resembling elasticity, accessibility for modification and robust mechanical performance. Their widely available and affordable raw components in-addition to straightforward synthesis and modification approach make hydrogels appealing material for flexible and wearable sensors in biomedical applications. This work demonstrates the development of new and sensitive material for strain sensing using polyvinyl alcohol (PVA) and κ-carrageenan (κCA) hydrogel comprising conductive polyaniline nanofibers (PANI NFs). The double-network hydrogel was produced via chemical crosslinking of PVA with Glutaraldehyde (GA) and physical crosslinking of κCA with potassium ions in a binary solvent system of deionized water and glycerol. The PANI NFs were then embedded in the hydrogel via the interfacial polymerization (IP) method of polyaniline nanofibers to significantly enhance the material properties and strain sensitivity of the pristine hydrogel. The obtained hydrogel has been involved in rigorous material characterization and sensing capability evaluation. The produced hydrogel demonstrated a high-water content (86.6%), high swelling percentage in acidic solutions, mechanical compressibility up to 60% at 400 kPa, high electrical conductivity of 2.11 S/m, and thermal stability ranging from − 26.9 to 120 oC. The hydrogel resulted in a linear response in its sensing performance of the applied stress (R2 = 0.99). Also, the developed composite demonstrated a sensitivity of 1.5 mV/kPa in stress range from zero up to 170 kPa with response and recovery times of ~ 300 ms and 500 ms, respectively.

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Hybrid Hydrogels with Orthogonal Transient Cross-linking Exhibiting Highly Tunable Mechanical Properties

Cited by 6 publications

References 48 publications

Cucurbit[8]uril Mediated Supramolecular and Photocrosslinked Interpenetrating Network Hydrogel Matrices for 3D‐Bioprinting

Cucurbit[8]uril Mediated Supramolecular and Photocrosslinked Interpenetrating Network Hydrogel Matrices for 3D‐Bioprinting

Supramolecular hydrogels based on hydrogen bonding: Impact of ionic comonomers

A new PVA-κCA double-network hydrogel comprising conductive polyaniline nanofibers for strain sensing applications

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